Description of molecular nanomagnets by the multi-orbital Hubbard model with correlated hopping

TL;DR

This paper models molecular nanomagnets using an advanced multi-orbital Hubbard approach that includes correlated hopping, providing insights into magnetic interactions, especially for the $Cr_8$ molecular ring, and demonstrating the impact of correlated hopping on magnetic coupling.

Contribution

It introduces a microscopic multi-orbital Hubbard model with correlated hopping for molecular magnets and derives the spin Hamiltonian, applying it specifically to the $Cr_8$ nanomagnet.

Findings

Correlated hopping reduces antiferromagnetic exchange in $Cr_8$.

The derived spin Hamiltonian matches spectral analysis results.

The method can be applied to various nanomagnets.

Abstract

We present a microscopic description of molecular magnets by the multi-orbital Hubbard model, which includes the correlated hopping term, i.e. the dependence of electron hopping amplitude between orbitals on the degree of their occupancy. In the limit of large Coulomb on-site interaction, we derived the spin Hamiltonian using the perturbation theory. The magnetic coupling constant between two ions we determined in two different ways: a)from the expression obtained in the perturbation calculus and b)from the analysis of distances between the lowest levels of the energy spectrum obtained by the diagonalization of the multi-orbital Hubbard model. The procedure we use can be applied to various nanomagnets, but the final calculations we performed for the molecular ring $Cr_8$. We showed that the correlated hopping can reduce the antiferromagnetic exchange between ions, what is essential for a proper description of $Cr_8$.